Fifth-order electronically non-resonant Raman scattering: two-dimensional Fourier deconvolution Original Research Article

This paper presents an analytical Fourier deconvolution procedure for homodyne detected electronically non-resonant fifth-order signal that reveals the bare nuclear response function free from the influence of the electronic (hyperpolarizability) responses generated by the five potentially overlapping finite duration pulses used in the experiment. In developing the fifth-order deconvolution procedure, an analogous procedure for homodyne detected third-order responses is elaborated. The potential implementation problems with the homodyne deconvolution procedure are evaluated through comparison of the third-order homodyne deconvolution result with that of the well-known third-order heterodyne deconvolution. Then, the homodyne deconvolution is extended to fifth-order where it is used on several measured tensor elements of the direct fifth-order signal. Suggestions are given for improving implementation of the procedure in fifth order so that more information on the direct fifth-order nuclear response as well as the hyperpolarizability responses can be recovered via the deconvolution procedure.